Electrooxidation of methane to acetic acid over ZnO nanosheets: Defect-sites engineering

Electrocatalytic conversion of methane (CH4) into high-valued liquid products have been studied extensively, yet still limited by their low product yields. Herein, we report the electrocatalytic conversion of CH4 into CH3COOH in HCO3--contained electrolyte. By optimizing the surface-active sites via defects engineering, a high CH3COOH yield of 347.31 mmol gcat-1 h-1, accompanied with a CH3COOH selectivity of 85.4 %, was obtained at 1.3 V vs RHE over the optimal catalyst. This CH3COOH yield is 2-5 orders of magnitude to previous reports so far as we know. Combinations of DFT theoretical simulation, defect sites characterization and control experiments of CH4 elec-trochemical conversion confirmed the important roles of ample surface Zn/O defects. Our work provides a new insight into the design of highly active and selective catalysts toward CH4 electrocatalytic conversion into CH3COOH.